Shortcut to Chemically Accurate Quantum Computing via Density-based Basis-set Correction

Abstract

Using GPU-accelerated state-vector emulation, we propose to embed a quantum computing ansatz into density-functional theory via density-based basis-set corrections (DBBSC) to obtain quantitative quantum-chemistry results on molecules that would otherwise require brute-force quantum calculations using hundreds of logical qubits. Indeed, accessing a quantitative description of chemical systems while minimizing quantum resources is an essential challenge given the limited qubit capabilities of current quantum processors. We provide a shortcut towards chemically accurate quantum computations by approaching the complete-basis-set limit through coupling the DBBSC approach, applied to any given variational ansatz, to an on-the-fly crafting of basis sets specifically adapted to a given system and user-defined qubit budget. The resulting approach self-consistently accelerates the basis-set convergence, improving electronic densities, ground-state energies, and first-order properties (e.g. dipole moments), but can also serve as a classical, a posteriori, energy correction to quantum hardware calculations with expected applications in drug design and materials science.

References in corpus (42)

• A variational eigenvalue solver on a quantum processor
• Hardware-efficient Variational Quantum Eigensolver for Small Molecules and Quantum Magnets
• The theory of variational hybrid quantum-classical algorithms
• Quantum computational chemistry
• Quantum Chemistry in the Age of Quantum Computing
• Simulated Quantum Computation of Molecular Energies
• The Variational Quantum Eigensolver: a review of methods and best practices
• An adaptive variational algorithm for exact molecular simulations on a quantum computer
• Quantum algorithms for quantum chemistry and quantum materials science
• Simulation of Electronic Structure Hamiltonians Using Quantum Computers
• qubit-ADAPT-VQE: An adaptive algorithm for constructing hardware-efficient ansatze on a quantum processor
• Quantum Package 2.0: An Open-Source Determinant-Driven Suite of Programs
• Qubit-excitation-based adaptive variational quantum eigensolver
• The Elephant in the Room of Density Functional Theory Calculations
• Quantum Algorithm for Molecular Properties and Geometry Optimization
• Quantum simulation of electronic structure with a transcorrelated Hamiltonian: improved accuracy with a smaller footprint on the quantum computer
• Similarity transformation of the electronic Schrödinger equation via Jastrow factorisation
• Curing basis-set convergence of wave-function theory using density-functional theory: a systematically improvable approach
• Almost exact energies for the Gaussian-2 set with the semistochastic heat-bath configuration interaction method
• Overlap-ADAPT-VQE: Practical Quantum Chemistry on Quantum Computers via Overlap-Guided Compact Ansätze
• Reducing qubit requirements while maintaining numerical precision for the Variational Quantum Eigensolver: A Basis-Set-Free Approach
• A Density-Based Basis-Set Correction For Wave Function Theory
• TETRIS-ADAPT-VQE: An adaptive algorithm that yields shallower, denser circuit ansätze
• Chemically Accurate Excitation Energies With Small Basis Sets
• A Density-Based Basis-Set Incompleteness Correction for GW Methods
• Communication: Curing basis set overcompleteness with pivoted Cholesky decompositions
• A basis-set error correction based on density-functional theory for strongly correlated molecular systems
• Improving the Accuracy of the Variational Quantum Eigensolver for Molecular Systems by the Explicitly-Correlated Perturbative [2]-R12-Correction
• TREXIO: A File Format and Library for Quantum Chemistry
• Avoiding symmetry roadblocks and minimizing the measurement overhead of adaptive variational quantum eigensolvers
• Explicitly correlated electronic structure calculations with transcorrelated matrix product operators
• Sparse Quantum State Preparation for Strongly Correlated Systems
• Extension of selected configuration interaction for transcorrelated methods
• Calculating the ground state energy of benzene under spatial deformations with noisy quantum computing
• Self-consistent density-based basis-set correction: How much do we lower total energies and improve dipole moments?
• Extension of the Trotterized Unitary Coupled Cluster to Triple Excitations
• Basis-set correction for coupled-cluster estimation of dipole moments
• Basis-set correction based on density-functional theory: Linear-response formalism for excited-state energies
• Basis-set correction based on density-functional theory: Rigorous framework for a one-dimensional model
• A density-fitting implementation of the density-based basis-set correction method
• Postponing the orthogonality catastrophe: efficient state preparation for electronic structure simulations on quantum devices
• Basis set generation and optimization in the NISQ era with Quiqbox.jl

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